CN1843575A - Method and apparatus for optic catalytic oxidizing, desulfurizing and denitrifying flue gas simultaneously - Google Patents
Method and apparatus for optic catalytic oxidizing, desulfurizing and denitrifying flue gas simultaneously Download PDFInfo
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- CN1843575A CN1843575A CNA2006100125267A CN200610012526A CN1843575A CN 1843575 A CN1843575 A CN 1843575A CN A2006100125267 A CNA2006100125267 A CN A2006100125267A CN 200610012526 A CN200610012526 A CN 200610012526A CN 1843575 A CN1843575 A CN 1843575A
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Abstract
The invention relates to a method for processing desulfuration and denitration simultaneously of smoke optical catalysis oxygenation and relative device, belonging to the smoke purifying technique. Said method comprises: guiding the coal-fired smoke into the reactor; filling optical catalyst into the reactor to be illuminated by light, while said optical catalyst is formed by carrier, and the titania and additive in 0.5% mass percentage; said carrier is quartz sand whose diameter is 4-6mm; said optical catalyst is the mixture of titania and the additive. The invention can complete the desulfuration and denitration simultaneously with high efficiency and stable operation, while it can apply the SO2 and NOx in different mass percentages, and the product can be used as muck; said desulfuration and denitration process will not generate pollution, with simple stricture and lower cost.
Description
Technical Field
The invention relates to a method and a device for desulfurizing and denitrating flue gas, in particular to a carrier type TiO2The photocatalyst catalyzes and oxidizes the flue gas so as to realize the desulfurization and denitrification of the flue gas, and belongs to the technical field of flue gas purification.
Background
SO generated in the process of burning coal in power plant2And NOXIs one of the main pollution sources causing air pollution at present, and the environmental problems caused by the pollution cause great attention worldwide, so the research on the flue gas desulfurization and denitration technology also becomes a research hotspot in the environmental field.
The current industrial methods for flue gas desulfurization can be divided into wet and dry processes. The traditional wet desulphurization process is a limestone-gypsum method, and although the process is mature, the equipment investment and the operation cost are high, and simultaneously, a large amount of desulphurization waste water is generated. Although the investment of equipment and the operation cost are reduced, the dry desulfurization process has the defects of unstable operation, limited flue gas removal amount and the like, so that the dry desulfurization process is greatly limited in practical application.
NOxMost of the removal studies of (1) are Selective Catalytic Reduction (SCR), which mostly uses ammonia as a reducing agent. Adding NOxReducing to nitrogen. The other is to oxidize the nitric acid into nitrate so as to remove NOxThe purpose of (1).
However, with respect to SO2And NOxThe simultaneous removal process has less research at home and abroad at present, and a plurality of SO2And NOxThe simultaneous removal process is only a simple combination of the desulfurization and denitrification processes, and does not really reach SO2And NOxThe purpose and effect of the removal are also achieved.
Chinese patent 03136387.3 discloses a catalytic desulfurization and denitrification method using TiO based on calcium carbonate2(La2O3、CeO2) Has the advantages ofAnd (4) desulfurizing and denitrating the absorbent with the catalytic oxidation function. However, in order to obtain higher catalytic oxidation efficiency, the method needs high-power ultraviolet irradiation, and the energy consumption is higher. And the desulfurization product of the method is CaSO4Insoluble in water and liable to block the channels, especially the catalyst TiO used in this process2(La2O3、CeO2) Cannot be recycled, and the method is expected to have huge running cost in practical engineering application.
Disclosure of Invention
The invention aims to provide a method and a device for realizing simultaneous desulfurization and denitrification of coal-fired flue gas by using a photocatalyst with low energy consumption and high efficiency.
The problems stated by the invention are solved by the following technical scheme:
a method for simultaneously carrying out photocatalytic oxidation, desulfurization and denitrification on flue gas comprises the following steps: introducing coal-fired flue gas into a reactor, filling a supported photocatalyst in the reactor, and performing light irradiation catalytic oxidation to complete the process of simultaneously desulfurizing and denitrifying the flue gas, wherein the photocatalyst consists of a granular carrier and titanium dioxide accounting for 0.5 percent of the mass of the carrier, and the supported photocatalyst is prepared by depositing and firing in photocatalyst deposition liquid added with an additive.
The method for simultaneously performing photocatalytic oxidation, desulfurization and denitrification on the flue gas comprises the steps that the additives are ZnO and Fe2O3、Al2O3And the like, metal oxides or metal Ag, and mixtures of the foregoing.
The method for simultaneously performing photocatalytic oxidation, desulfurization and denitrification on the flue gas adds a catalyst regeneration process after the catalytic oxidation process, washes the inactivated photocatalyst by using water, and removes HNO on the surface of the photocatalyst3And H2SO4And (4) removing.
The method for simultaneously performing photocatalytic oxidation, desulfurization and denitrification on the flue gas comprises the following steps:
a. preparing photocatalyst deposition liquid: 0.1mol/L ammonium fluorotitanate ((NH) was prepared4)2TiF6) Solution and 0.3mol/L boric acid (H)3BO3) Uniformly mixing the solution to prepare photocatalyst deposition solution, and adding an additive with the mass ratio of 0.5-10%;
b. deposition: immersing the carrier in the deposition solution for 40-50 hours at the temperature of 40 ℃ in a water bath, and then taking out and airing;
c. firing: heating to 450 ℃ at the heating rate of 10 ℃/min, and burning for 30 minutes to obtain the supported titanium dioxide photocatalyst.
According to the method for simultaneously performing photocatalytic oxidation, desulfurization and denitrification on the flue gas, the humidity of the photocatalytic reaction is 3% -10%, and the temperature is 60-120 ℃.
According to the method for simultaneously performing photocatalytic oxidation, desulfurization and denitrification on the flue gas, the carrier is quartz sand, and the particle size of the quartz sand is 4-6 mm.
The utility model provides a flue gas photocatalytic oxidation device of SOx/NOx control simultaneously, it comprises reactor 1, temperature regulator 9, steam generator 11 and absorber 5, be equipped with light source 6(60W fluorescent tube) and fill load type photocatalyst 12 in the reactor, the carrier is quartz sand, and its particle diameter is 4 ~ 6mm, the photocatalyst is the mixture of titanium dioxide and additive, is equipped with into mouth 8, steam entry 10 and discharge gate 7 in the reactor bottom, and reactor upper portion is equipped with material filling port 2 and outlet flue 4, temperature regulator communicates in inlet flue department, steam generator even leads to the steam entry, outlet flue intercommunication absorber.
Above-mentioned flue gas photocatalytic oxidation SOx/NOx control's device simultaneously, be equipped with the light source protective sheath around the light source.
The invention has the following advantages: first, the present invention can simultaneously complete desulfurization and denitrification, and is not a simple combination of conventional desulfurization and denitrification processes. The method completes the two processes by using the photocatalyst, has high efficiency and stable operation, and is suitable for the flue gas with different component contents. Second, the apparatus of the present invention promotes an increase in the efficiency of photocatalytic oxidation. The steam generator can provide the amount of steam required by the photocatalytic oxidation reaction and can be used according to the amount of the photocatalyst and SO2And NOxThe concentration is adjusted. Particle size of Quartz Sand CarrierModerate, not only can improve the adsorption quantity of the photocatalyst to gas, but also can increase the transmission ratio of ultraviolet light, thereby enlarging the formation of electron-hole pairs. Thirdly, the products of desulfurization and denitrification absorbed by ammonia water are ammonium sulfate and ammonium nitrate, and the recovered products can be used as fertilizers. The process steps accord with the principle of circular economy, and the photocatalyst has low consumption and long service life, can be repeatedly used, particularly does not generate substances which are toxic and harmful to the environment in the catalysis process, and is a very environment-friendly method. Fourth, the inventive device structureSimple structure, low manufacturing cost, cheap and easily obtained carrier raw materials and convenient popularization and application. Fifth, high SO concentrations can be achieved2And NOxSimultaneously removing SO under the conditionthat the loading amount of the photocatalyst is 5g/kg2The concentration is 1500-5000 mg/m3In the range of 100% desulfurization efficiency, NOxThe concentration is 600-1300 mg/m3The removal efficiency is more than 55 percent in the range.
Drawings
FIG. 1 is a schematic view of the structure of an apparatus used in the present invention;
FIG. 2 is a process flow diagram of the present invention.
The numbers in the figures are as follows: 1. a reactor; 2. a feeding port; 3. a light source protective sleeve; 4. a smoke outlet; 5. an absorber; 6. a light source; 7. a discharge port; 8. a smoke inlet; 9. a temperature regulator; 10. a water vapor inlet; 11. a water vapor generator; 12. a photocatalyst.
Detailed Description
Referring to FIG. 2, the present invention provides a purification method in which a photocatalyst is added to a reactor. The photocatalyst is used for photocatalytic oxidation and absorption of SO in the flue gas under the conditions that the humidity of the flue gas is 3-10% and the temperature is 50-120 DEG C2And NOxOxidizing it to SO4 2-And NO3 -And is converted into ammonium sulfate and ammonium nitrate by an absorption device added with ammonia water, thereby removing SO in the flue gas2And NOx.
Photo catalysisThe catalyst consists of a carrier, 0.5 percent of titanium dioxide and an additive, wherein the carrier is required to have a large specific surface area so as to load the photocatalyst; the photocatalyst adopts a mixture of titanium dioxide and additives, wherein theadditives comprise ZnO and Fe2O3、Al2O3And the like metal oxides and metal Ag.
The photocatalyst after use can recover the catalytic activity after being washed and purified by water.
The main reactions of photocatalytic oxidation are:
(1) photocatalytic desulfurization reaction
(2) Photocatalytic denitration reaction
Or
The last step is to remove HNO from the surface of the photocatalyst by water3And H2SO4A compound to regenerate the photocatalyst.
The photocatalyst carrier in the invention is granular quartz sand with the grain diameter of 4-6 mm. The carrier type photocatalyst can overcome powdered TiO2The photocatalyst has the defects of difficult separation, large using amount, low optical activity, short service life, need of good regeneration technology and the like, and simultaneously can adsorb more SO on the surface of the photocatalyst due to large specific surface area2And NOxThe photocatalytic efficiency is improved. The carrier type photocatalyst forms an electron accumulation center on the surface of the photocatalyst under the action of the additive, and the electron accumulation center is aligned with TiO2The free electrons form the best attraction, thereby increasing the separation probability of photo-generated electrons and holes, leading the photocatalyst to have higher catalytic activity, generating more strong oxidizing free radicals under the participation of additives and oxygen, and being capable of treating SO2And NOxThe oxidation is more complete.
Referring to fig. 1, the apparatus used in the present invention comprises a photocatalytic reactor 1, a temperature regulator 9, a water vapor generator 11, and an absorber 5. The bottom of the photocatalytic reactor 1 is provided with a smoke inlet 8, a vapor inlet 10 and a discharge hole 7, the upper part is provided with a smoke outlet 4 and a feeding hole 2, and a light source 6(60W fluorescent tube), a light source protective sleeve 3 and a photocatalyst 12 are arranged inside the photocatalytic reactor. The smoke outlet 4 is connected with an absorber 5. The flue gas enters the temperature regulator 12 through the pipeline and then enters through the flue gas inlet 8. Steam is generated from the steam generator 11 and injected through the steam inlet 10 for providing the steam required for the photocatalytic reaction. The amount of steam can be determined by the amount of photocatalyst and SO2And NOxIs adjusted. The humidity inside the reactor is maintained at 3-10 wt% and the temperature is maintained at 60-120 deg.c.
In the preparation process of the photocatalyst, the additive is doped in the titanium dioxide, so that the photoelectron utilization rate of the photocatalyst is improved, the light source adopts a common fluorescent lamp tube, the light source cost is reduced, the problem of ultraviolet leakage caused by the utilization of an ultraviolet light source by other reactors is solved, and the process safety is improved.
Several specific examples are provided below:
example 1:
0.1mol/L ammonium fluorotitanate ((NH) was prepared4)2TIF6) And 0.3mol/L boric acid (H)3BO3) The mixed solution is photocatalyst deposition solution, ZnO additive with the mass ratio of 0.5 percent is added into the deposition solution, the mixture is deposited on carrier quartz sand with the grain diameter of 4-6mm under the condition of water bath at 40 ℃, the carrier quartz sand is taken out after 45 hours and dried, the temperature is raised to 450 ℃ at the heating rate of 10 ℃/min and is burnt for 30 minutes,thus obtaining the supported TiO2A photocatalyst. The catalytic reaction conditions are as follows: the humidity was 3% and the temperature was 70 ℃.
Example 2
0.1mol/L ammonium fluorotitanate ((NH) was prepared4)2TIF6) And 0.3mol/L boric acid (H)3BO3) Photocatalyst deposition solution is added with 0.5 percent of Fe2O3Depositing an additive on carrier quartz sand with the particle size of 4-6mm under the condition of water bath at 40 ℃, taking out the carrier quartz sand after 40 hours, drying the carrier quartz sand, raising the temperature to 450 ℃ at the heating rate of 10 ℃/min, and firing the carrier quartz sand for 30 minutes to obtain the supported TiO2A photocatalyst. The catalytic reaction conditions are as follows: the humidity was 10% and the temperature was 60 ℃.
Example 3
0.1mol/L ammonium fluotitanate (NH) is prepared4)2TIF6And 0.3mol/L boric acid H3BO3Photocatalyst deposition liquid is added with 0.5 percent of Al2O3Depositing an additive on carrier quartz sand with the particle size of 4-6mm under the condition of water bath at 40 ℃, taking out and drying after 45 hours, raising the temperature to 450 ℃ at the heating rate of 10 ℃/min, and firing for 30 minutes to obtain the supported TiO2A photocatalyst. The catalytic reaction conditions are as follows: the humidity was 6% and the temperature was 120 ℃.
Example 4
0.1mol/L ammonium fluorotitanate ((NH) was prepared4)2TIF6) And 0.3mol/L boric acid (H)3BO3) The mixed solution is photocatalyst deposition solution, and is added into the deposition solutionIntroduction of 10% AgNO3Depositing an additive on carrier quartz sand with the particle size of 4-6mm under the condition of water bath at 40 ℃, taking out and drying after 45 hours, raising the temperature to 450 ℃ at the heating rate of 10 ℃/min, and firing for 30 minutes to obtain the supported TiO2A photocatalyst. The catalytic reaction conditions are as follows: the humidity was 8% and the temperature was 95 ℃.
Example 5
0.1mol/L ammonium fluorotitanate ((NH) was prepared4)2TIF6) And 0.3mol/L boric acid (H)3BO3) The mixed solution is photocatalyst deposition solution, and 0.5% Al is added into the deposition solution2O3And 5% AgNO3Depositing an additive on carrier quartz sand with the particle size of 4-6mm under the condition of water bath at 40 ℃, taking out and drying after 45 hours, raising the temperature to 450 ℃ at the heating rate of 10 ℃/min, and firing for 30 minutes to obtain the supported TiO2A photocatalyst. The catalytic reaction conditions are as follows: the humidity was 9% and the temperature was 110 ℃.
Claims (8)
1. A method for simultaneously performing photocatalytic oxidation, desulfurization and denitrification on flue gas is characterized by comprising the following steps: the method comprises the following steps: introducing coal-fired flue gas into a reactor, filling a supported photocatalyst in the reactor, and irradiating and catalyzing the reactor by light to complete the process of simultaneously desulfurizing and denitrifying the flue gas, wherein the photocatalyst consists of a granular carrier and titanium dioxide accounting for 0.5 percent of the mass of the carrier, and the supported photocatalyst is prepared by depositing and firing in photocatalyst deposition liquid added with an additive.
2. The method for simultaneously performing photocatalytic oxidation, desulfurization and denitrification on flue gas according to claim 1, is characterized in that: the additive is ZnO or Fe2O3、Al2O3And the like, metal oxides or metal Ag, and mixtures of the foregoing.
3. The method for simultaneously performing photocatalytic oxidation, desulfurization and denitrification on flue gas according to claim 2, is characterized in that: adding catalyst regeneration process after catalytic oxidation process, and flushing with waterWashing the deactivated photocatalyst to remove HNO on the surface of the photocatalyst3And H2SO4And (4) removing.
4. The method for simultaneously performing photocatalytic oxidation, desulfurization and denitrification on flue gas according to claim 3, is characterized in that: the photocatalyst is prepared by the following steps:
a. preparing photocatalyst deposition liquid: 0.1mol/L ammonium fluotitanate solution and 0.3mol/L boric acid solution are evenly mixed to prepare photocatalyst deposition solution, and 0.5 to 10 mass percent of additive is added;
b. deposition: immersing the carrier in the deposition solution for 40-50 hours at the temperature of 40 ℃ in a water bath, and then taking out and airing;
c. firing: heating to 450 ℃ at the heating rate of 10 ℃/min, and burning for 30 minutes to obtain the supported titanium dioxide photocatalyst.
5. The method for simultaneously performing photocatalytic oxidation, desulfurization and denitrification on flue gas according to claim 4, is characterized in that: the humidity of the photocatalytic reaction is 3% -10%, and the temperature is 60-120 ℃.
6. The method for simultaneously performing photocatalytic oxidation, desulfurization and denitrification on flue gas according to claim 5, is characterized in that: the granular carrier is quartz sand, and the particle size of the granular carrier is4-6 mm.
7. The utility model provides a flue gas photocatalytic oxidation while SOx/NOx control's device which characterized in that: it comprises reactor (1), temperature regulator (9), steam generator (11) and absorber (5), inside light source (6) of being equipped with of reactor to fill load type photocatalyst (12), the carrier is quartz sand, and its particle diameter is 4 ~ 6mm, the photocatalyst is the mixture of titanium dioxide and additive, and the reactor bottom is equipped with into mouth (8), steam entry (10) and discharge gate (7), and reactor upper portion is equipped with material adding mouth (2) and outlet flue (4), temperature regulator communicates in inlet flue department, steam generator links to each other the steam entry, outlet flue intercommunication absorber.
8. The device for simultaneously performing photocatalytic oxidation, desulfurization and denitrification on flue gas according to claim 7, is characterized in that: and a light source protective sleeve is arranged around the light source.
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| CN101955193A (en) * | 2010-09-16 | 2011-01-26 | 上海电力学院 | Method for preparing hydrogen and fertilizer ammonium sulfate by desulfurizing coal-fired waste gas |
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| CN102000503A (en) * | 2010-12-10 | 2011-04-06 | 武汉慧邦环境工程技术有限公司 | Photocatalytic oxidation flue gas desulfurization and denitration system of coal-fired power plant |
| CN101322903B (en) * | 2008-07-11 | 2011-07-20 | 南京工业大学 | Gas desulfurization and denitration method |
| CN102335539A (en) * | 2011-09-06 | 2012-02-01 | 江苏华正环保科技有限公司 | Process for removing tobacco odour |
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| CN101961601B (en) * | 2010-09-03 | 2012-08-22 | 武汉慧邦环境工程技术有限公司 | Waste gas purification system of photocatalytic filter tower |
| CN101955193B (en) * | 2010-09-16 | 2012-06-20 | 上海电力学院 | Method for preparing hydrogen and fertilizer ammonium sulfate by desulfurizing coal-fired waste gas |
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